US9096725B2ActiveUtilityA1

Cross-linked polyazole, method of preparing the polyazole, electrode for fuel cell including the cross-linked polyazole, electrolyte membrane for fuel cell including the cross-linked polyazole, method of manufacturing the electrolyte membrane, and fuel cell including the cross-linked polyazole

78
Assignee: CHOI SEONG-WOOPriority: Apr 24, 2009Filed: Apr 23, 2010Granted: Aug 4, 2015
Est. expiryApr 24, 2029(~2.8 yrs left)· nominal 20-yr term from priority
C08J 5/2256H01M 8/1081C08G 73/18H01M 8/1072C08L 65/00C08L 79/04C08G 2261/312C08G 61/12C08K 5/357C08G 2261/592C08G 2261/62H01M 8/1048C08G 2261/598C08G 2261/3241Y02E60/521H01M 8/103C08G 2261/516C08G 2261/126H01M 8/1088H01M 8/1027C08J 2379/06Y02E60/50Y02P70/50
78
PatentIndex Score
2
Cited by
39
References
43
Claims

Abstract

A cross-linked polyazole, a method of preparing the cross-linked polyazole, an electrode and an electrolyte membrane for a fuel cell, which include the cross-linked polyazole, a method of manufacturing the electrolyte membrane, and a fuel cell including the cross-linked polyazole.

Claims

exact text as granted — not AI-modified
What is claimed is: 
     
       1. A composition comprising: a polyazole including a first repeating unit comprising a repeating unit represented by one of the following formulas: 
       
         
           
           
               
               
           
         
         wherein Ar is selected from among the following groups: 
       
       
         
           
           
               
               
           
         
       
       an azole second repeating unit having at least one amino group; and a benzoxazine-based monomer, wherein, assuming that m and n represent the relative molar amount of the first repeating unit and the azole second repeating unit, respectively, in the polyazole such that m+n=1, m ranges from 0.1 to 0.9 and n ranges from 0.1 to 0.9:
 and 
 wherein the azole second repeating unit comprises a repeating unit represented by 
 
       
         
           
           
               
               
           
         
         wherein, in Formula 2a, R 3 , R 3 ′, R 3 ″, R 3 ′″, R 4 , R 4 ′, R 4 ″, R 5 , R 5 ′, and R 5 ″ are each independently a hydrogen atom, an unsubstituted or substituted C1-C20 alkyl group, an unsubstituted or substituted C1-C20 alkoxy group, an unsubstituted or substituted C6-C20 aryl group, an unsubstituted or substituted C6-C20 aryloxy group, an unsubstituted or substituted C3-C20 heteroaryl group, or an unsubstituted or substituted C3-C20 heteroaryloxy group, wherein R 1  and R 2  may be linked to form a C4-C20 carbon ring or a C3-C20 hetero ring; and 
         L represents a linker. 
       
     
     
       2. The composition of  claim 1 , wherein the amount of the polyazole is in the range of about 40 parts to about 210 parts by weight based on 100 parts by weight of the benzoxazine-based monomer. 
     
     
       3. The composition of  claim 1 , wherein L in Formula 2a is —CH 2 —, —C(CH 3 ) 2 —, or —C(CF 3 ) 2 —. 
     
     
       4. The composition of  claim 1 , wherein the polyazole is a block copolymer including the first repeating unit and the second repeating unit of Formula 2a. 
     
     
       5. The composition of  claim 1 , wherein the polyazole has a degree of polymerization of about 1 to about 900. 
     
     
       6. The composition of  claim 1 , wherein the polyazole comprises a block copolymer represented by Formula 3 below: 
       
         
           
           
               
               
           
         
         wherein, in Formula 3, R 1 , R 1 ′ and R 2  are hydrogen; 
         Ar is selected from among the following groups: 
       
       
         
           
           
               
               
           
         
         m is a number from 0.1 to 0.9; 
         a is 1; 
         R 3 , R 3 ′, R 3 ″, R 3 ′″, R 4 , R 4 ′, R 4 ″, R 5 , R 5 ′, and R 5 ″ are each independently a hydrogen atom, an unsubstituted or substituted C1-C20 alkyl group, an unsubstituted or substituted C1-C20 alkoxy group, an unsubstituted or substituted C6-C20 aryl group, an unsubstituted or substituted C6-C20 aryloxy group, an unsubstituted or substituted C3-C20 heteroaryl group, or an unsubstituted or substituted C3-C20 heteroaryloxy group, wherein R 1  and R 2  may be linked to form a C4-C20 carbon ring or a C3-C20 hetero ring; 
         L represents a linker; 
         n is a number from greater than 0 to 0.99; and 
         k represents a degree of polymerization of the polyazole and is a number from 10 to 300. 
       
     
     
       7. The composition of  claim 1 , wherein the benzoxazine-based monomer comprises at least one compound selected from among the compounds represented by Formulae 6 through 11 below: 
       
         
           
           
               
               
           
         
         in Formula 6, R 1  through R 4  are each independently a hydrogen atom, a substituted or unsubstituted C 1 -C 20  alkyl group, a substituted or unsubstituted C 1 -C 20  alkoxy group, a substituted or unsubstituted C 2 -C 20  alkenyl group, a substituted or unsubstituted C 2 -C 20  alkynyl group, a substituted or unsubstituted C 6 -C 20  aryl group, a substituted or unsubstituted C 6 -C 20  aryloxy group, a substituted or unsubstituted C 2 -C 20  heteroaryl group, a substituted or unsubstituted C 2 -C 20  heteroaryloxy group, a substituted or unsubstituted C 4 -C 20  carbon ring group, a substituted or unsubstituted C 4 -C 20  carbocyclic alkyl group, a substituted or unsubstituted C 2 -C 20  heterocyclic group, a halogen atom, a hydroxyl group, or a cyano group; and 
         R 5  is a substituted or unsubstituted C 1 -C 20  alkyl group, a substituted or unsubstituted C 1 -C 20  alkoxy group, a substituted or unsubstituted C 2 -C 20  alkenyl group, a substituted or unsubstituted C 2 -C 20  alkynyl group, a substituted or unsubstituted C 6 -C 20  aryl group, a substituted or unsubstituted C 6 -C 20  aryloxy group, a substituted or unsubstituted C 7 -C 20  arylalkyl group, a substituted or unsubstituted C 2 -C 20  heteroaryl group, a substituted or unsubstituted C 2 -C 20  heteroaryloxy group, a substituted or unsubstituted C 2 -C 20  heteroarylalkyl group, a substituted or unsubstituted C 4 -C 20  carbocyclic group, a substituted or unsubstituted C 4 -C 20  carbocyclic alkyl group, a substituted or unsubstituted C 2 -C 20  heterocyclic group, or a substituted or unsubstituted C 2 -C 20  heterocyclic alkyl group, 
       
       
         
           
           
               
               
           
         
         in Formula 7, R 5 ′ is a substituted or unsubstituted C 1 -C 20  alkyl group, a substituted or unsubstituted C 1 -C 20  alkoxy group, a substituted or unsubstituted C 2 -C 20  alkenyl group, a substituted or unsubstituted C 2 -C 20  alkynyl group, a substituted or unsubstituted C 6 -C 20  aryl group, a substituted or unsubstituted C 6 -C 20  aryloxy group, a substituted or unsubstituted C 7 -C 20  arylalkyl group, a substituted or unsubstituted C 2 -C 20  heteroaryl group, a substituted or unsubstituted C 2 -C 20  heteroaryloxy group, a substituted or unsubstituted C 2 -C 20  heteroarylalkyl group, a substituted or unsubstituted C 4 -C 20  carbocyclic group, a substituted or unsubstituted C 4 -C 20  carbocyclic alkyl group, a substituted or unsubstituted C 2 -C 20  heterocyclic group, or a substituted or unsubstituted C 2 -C 20  heterocyclic alkyl group; and 
         R 6  is selected from the group consisting of a substituted or unsubstituted C 1 -C 20  alkylene group, a substituted or unsubstituted C 2 -C 20  alkenylene group, a substituted or unsubstituted C 2 -C 20  alkynylene group, a substituted or unsubstituted C 6 -C 20  arylene group, a substituted or unsubstituted C 2 -C 20  heteroarylene group, —C(═O)—, and —SO 2 —, 
       
       
         
           
           
               
               
           
         
         in Formula 8, A, B, C, D and E are all carbon; or one or two of A, B, C, D and E is nitrogen and the others are carbon; and 
         R 1  and R 2  are linked to form a ring, wherein the ring is a C 6 -C 10  carbon ring group, a C 3 -C 10  heteroaryl group, a fused C 3 -C 10  heteroaryl group, a C 3 -C 10  heterocyclic group or a fused C 3 -C 10  heterocyclic group; 
       
       
         
           
           
               
               
           
         
         in Formula 9, A is a substituted or unsubstituted C 1 -C 20  heterocyclic group, a substituted or unsubstituted C 4 -C 20  cycloalkyl group, or a substituted C 1 -C 20  alkyl group, and wherein A includes at least one oxazine moiety; and 
         R 1  through R 8  are each independently a hydrogen atom, a C 1 -C 20  alkyl group, a C 1 -C 20  alkoxy group, a C 6 -C 20  aryl group, a C 6 -C 20  aryloxy group, a C 1 -C 20  heteroaryl group, a C 1 -C 20  heteroaryloxy group, a C 4 -C 20  cycloalkyl group, a C 1 -C 20  heterocyclic group, a halogen atom, a cyano group, or a hydroxy group, 
       
       
         
           
           
               
               
           
         
         in Formula 10, R 1  and R 2  are each independently a C 1 -C 20  alkyl group, a C 1 -C 20  alkoxy group, a C 6 -C 20  aryl group, a C 6 -C 20  aryloxy group or a group represented by Formula 10A below, 
       
       
         
           
           
               
               
           
         
         in Formulae 10 and 10A, R 3  is a hydrogen atom, a C 1 -C 20  alkyl group, a C 1 -C 20  alkoxy group, a C 6 -C 20  aryl group, a C 6 -C 20  aryloxy group, a halogenated C 6 -C 20  aryl group, a halogenated C 6 -C 20  aryloxy group, a C 1 -C 20  heteroaryl group, a C 1 -C 20  heteroaryloxy group, a halogenated C 1 -C 20  heteroaryl group, a halogenated C 1 -C 20  heteroaryloxy group, a C 4 -C 20  carbon ring group, a halogenated C 4 -C 20  carbon ring group, a C 1 -C 20  heterocyclic group or a halogenated C 1 -C 20  heterocyclic group, 
       
       
         
           
           
               
               
           
         
         in Formula 11, at least two adjacent groups selected from among R 2 , R 3  and R 4  are linked to form a group represented by Formula 12A below, and the non-selected, remaining group is a hydrogen atom, a C 1 -C 20  alkyl group, a C 1 -C 20  alkoxy group, a C 6 -C 20  aryl group, a C 6 -C 20  aryloxy group, a halogenated C 6 -C 20  aryl group, a halogenated C 6 -C 20  aryloxy group, a C 1 -C 20  heteroaryl group, a C 1 -C 20  heteroaryloxy group, a halogenated C 1 -C 20  heteroaryl group, a halogenated C 1 -C 20  heteroaryloxy group, a C 4 -C 20  carbon ring group, a halogenated C 4 -C 20  carbon ring group, a C 1 -C 20  heterocyclic group or a halogenated C 1 -C 20  heterocyclic group; and 
         at least two adjacent groups selected from among R 5 , R 6  and R 7  are linked to form the group represented by Formula 12A below, and the non-selected, remaining group is a C 1 -C 20  alkyl group, a C 1 -C 20  alkoxy group, a C 6 -C 20  aryl group, a C 6 -C 20  aryloxy group, a halogenated C 6 -C 20  aryl group, a halogenated C 6 -C 20  aryloxy group, a C 1 -C 20  heteroaryl group, a C 1 -C 20  heteroaryloxy group, a halogenated C 1 -C 20  heteroaryl group, a halogenated C 1 -C 20  heteroaryloxy group, a C 4 -C 20  carbon ring group, a halogenated C 4 -C 20  carbon ring group, a C 1 -C 20  heterocyclic group or a halogenated C 1 -C 20  heterocyclic group, and 
       
       
         
           
           
               
               
           
         
         in Formula 12A, R 1  is a substituted or unsubstituted C 1 -C 20  alkyl group, a substituted or unsubstituted C 1 -C 20  alkoxy group, a substituted or unsubstituted C 2 -C 20  alkenyl group, a substituted or unsubstituted C 2 -C 20  alkynyl group, a substituted or unsubstituted C 6 -C 20  aryl group, a substituted or unsubstituted C 6 -C 20  aryloxy group, a substituted or unsubstituted C 7 -C 20  arylalkyl group, a substituted or unsubstituted C 2 -C 20  heteroaryl group, a substituted or unsubstituted C 2 -C 20  heteroaryloxy group, a substituted or unsubstituted C 2 -C 20  heteroarylalkyl group, a substituted or unsubstituted C 4 -C 20  carbon ring group, a substituted or unsubstituted C 4 -C 20  carbocyclic alkyl group, a substituted or unsubstituted C 2 -C 20  heterocyclic group, or a substituted or unsubstituted C 2 -C 20  heterocyclic alkyl group; and 
         * denotes the sites at which the at least two adjacent groups selected from among R 2 , R 3  and R 4  of Formula 11 and the at least two adjacent groups selected from among R 5 , R 6  and R 7  are linked, respectively. 
       
     
     
       8. A cross-linked polyazole obtained through a cross-linking reaction of the composition of  claim 1 . 
     
     
       9. A method of preparing the cross-linked polyazole of  claim 8 , the method comprising:
 mixing a polyazole including a first repeating unit comprising a repeating unit represented by one of the following formulas: 
 
       
         
           
           
               
               
           
         
         wherein Ar is selected from among the following groups: 
       
       
         
           
           
               
               
           
         
       
       an azole second repeating unit having at least one amino group, a benzoxazine-based monomer and a phosphoric acid-based material to obtain a mixture, wherein, assuming that m and n represent the relative molar amount of the first repeating unit and the azole second repeating unit, respectively, in the polyazole such that m+n=1, m ranges from 0.1 to 0.9 and n ranges from 0.1 to 0.9; and
 thermally treating the mixture, 
 wherein the azole second repeating unit comprises a repeating unit represented by 
 
       
         
           
           
               
               
           
         
         wherein, in Formula 2a, R 3 , R 3 ′, R 3 ″, R 3 ′″, R 4 , R 4 ′, R 4 ″, R 5 , R 5 ′, and R 5 ″ are each independently a hydrogen atom, an unsubstituted or substituted C1-C20 alkyl group, an unsubstituted or substituted C1-C20 alkoxy group, an unsubstituted or substituted C6-C20 aryl group, an unsubstituted or substituted C6-C20 aryloxy group, an unsubstituted or substituted C3-C20 heteroaryl group, or an unsubstituted or substituted C3-C20 heteroaryloxy group, wherein R 1  and R 2  may be linked to form a C4-C20 carbon ring or a C3-C20 hetero ring; and 
         L represents a linker. 
       
     
     
       10. The method of  claim 9 , wherein the thermally treating is performed at a temperature of about 60 to about 250° C. 
     
     
       11. The method of  claim 9 , wherein the phosphoric acid-based material comprises at least one material selected from the group consisting of polyphosphoric acid, phosphonic acid (H 3 PO 3 ), ortho-phosphoric acid (H 3 PO 4 ), pyro-phosphoric acid (H 4 P 2 O 7 ), triphosphoric acid (H 5 P 3 O 10 ), meta-phosphoric acid, and a derivative thereof. 
     
     
       12. The method of  claim 9 , wherein the polyazole including the first repeating unit and the azole second repeating unit having at least one amino group is prepared through polymerization using a material that generates phosphoric acid when hydrolyzed. 
     
     
       13. The method of  claim 12 , wherein the material that generates phosphoric acid when hydrolyzed comprises polyphosphoric acid. 
     
     
       14. The method of  claim 9 , wherein the polyazole including the first repeating unit and the azole second repeating unit having at least one amino group is prepared by a method comprising:
 mixing biphenyl-3,3′,4,4′-tetraaminetetrahydrochloride and phosphoric acid, and thermally treating the mixture at a temperature of about 60 to about 250° C. to obtain a (2,2-(m-phenylene)-5,5-bibenzimidazole) oligomer; and 
 mixing the (2,2-(m-phenylene)-5,5-bibenzimidazole) oligomer with 3,4-diaminobenzoic acid and thermally treating the mixture at a temperature of about 60 to about 250° C. 
 
     
     
       15. An electrolyte membrane for a fuel cell, the electrolyte membrane comprising a composition comprising: a polyazole including a first repeating unit comprising a repeating unit represented by one of the following formulas: 
       
         
           
           
               
               
           
         
         wherein Ar is selected from among the following groups: 
       
       
         
           
           
               
               
           
         
       
       an azole second repeating unit; and a benzoxazine-based monomer, wherein, assuming that m and n represent the relative molar amount of the first repeating unit and the azole second repeating unit, respectively, in the polyazole such that m+n=1, m is a number from 0.1 to 0.9 and n is a number from 0.1 to 0.9:
 and wherein the azole second repeating unit comprises a repeating unit represented by Formula 2a: 
 
       
         
           
           
               
               
           
         
         wherein, in Formula 2a, R 3 , R 3 ′, R 3 ″, R 3 ′″, R 4 , R 4 ′, R 4 ″, R 5 , R 5 ′, and R 5 ″ are each independently a hydrogen atom, an unsubstituted or substituted C1-C20 alkyl group, an unsubstituted or substituted C1-C20 alkoxy group, an unsubstituted or substituted C6-C20 aryl group, an unsubstituted or substituted C6-C20 aryloxy group, an unsubstituted or substituted C3-C20 heteroaryl group, or an unsubstituted or substituted C3-C20 heteroaryloxy group, wherein R 1  and R 2  may be linked to form a C4-C20 carbon ring or a C3-C20 hetero ring; and 
         L represents a linker. 
       
     
     
       16. An electrolyte membrane for a fuel cell, the electrolyte membrane comprising a cross-linked polyazole obtained through a cross-linking reaction of a composition comprising: a polyazole including a first repeating unit comprising a repeating unit represented by one of the following formulae: 
       
         
           
           
               
               
           
         
         wherein Ar is selected from among the following groups: 
       
       
         
           
           
               
               
           
         
       
       an azole second repeating unit; and a benzoxazine-based monomer, wherein, assuming that m and n represent the relative molar amount of the first repeating unit and the azole second repeating unit, respectively, in the polyazole such that m+n=1, m is a number from 0.1 to 0.9 and n is a number from 0.1 to 0.9;
 and 
 wherein the azole second repeating unit comprises a repeating unit represented by Formula 2a: 
 
       
         
           
           
               
               
           
         
         wherein, in Formula 2a, R 3 , R 3 ′, R 3 ″, R 3 ′″, R 4 , R 4 ′, R 4 ″, R 5 , R 5 ′, and R 5 ″ are each independently a hydrogen atom, an unsubstituted or substituted C1-C20 alkyl group, an unsubstituted or substituted C1-C20 alkoxy group, an unsubstituted or substituted C6-C20 aryl group, an unsubstituted or substituted C6-C20 aryloxy group, an unsubstituted or substituted C3-C20 heteroaryl group, or an unsubstituted or substituted C3-C20 heteroaryloxy group, wherein R 1  and R 2  may be linked to form a C4-C20 carbon ring or a C3-C20 hetero ring; and 
         L represents a linker. 
       
     
     
       17. A method of manufacturing an electrolyte membrane for a fuel cell of  claim 16 , the method comprising:
 mixing a polyazole including a first repeating unit comprising a repeating unit represented by one of the following formulae: 
 
       
         
           
           
               
               
           
         
         wherein Ar is selected from among the following groups: 
       
       
         
           
           
               
               
           
         
       
       an azole second repeating unit having at least one amino group, a benzoxazine-based monomer and a phosphoric acid-based material to obtain a mixture, wherein, assuming that m and n represent the relative molar amount of the first repeating unit and the azole second repeating unit, respectively, in the polyazole such that m+n=1, m ranges from 0.1 to 0.9 and n ranges from 0.1 to 0.9;
 casting the mixture on a substrate and thermally treating the cast mixture to obtain a thermally-treated product; 
 impregnating the thermally-treated product with the phosphoric acid-based material to obtain a resulting product; and 
 drying the resulting product, 
 wherein the azole second repeating unit comprises a repeating unit represented by Formula 2a: 
 
       
         
           
           
               
               
           
         
         wherein, in Formula 2a, R 3 , R 3 ′, R 3 ″, R 3 ′″, R 4 , R 4 ′, R 4 ″, R 5 , R 5 ′, and R 5 ″ are each independently a hydrogen atom, an unsubstituted or substituted C1-C20 alkyl group, an unsubstituted or substituted C1-C20 alkoxy group, an unsubstituted or substituted C6-C20 aryl group, an unsubstituted or substituted C6-C20 aryloxy group, an unsubstituted or substituted C3-C20 heteroaryl group, or an unsubstituted or substituted C3-C20 heteroaryloxy group, wherein R 1  and R 2  may be linked to form a C4-C20 carbon ring or a C3-C20 hetero ring; and 
         L represents a linker. 
       
     
     
       18. The method of  claim 17 , further comprising treating the thermally-treated product in a constant-temperature and constant humidity condition at a temperature of about −20 to about 30° C. and a relative humidity of about 5 to about 50%. 
     
     
       19. The method of  claim 17 , wherein, the mixing of the polyazole including the first repeating unit and the azole second repeating unit having at least one amino group, the benzoxazine-based monomer and the phosphoric acid-based material comprises: mixing the polyazole with the phosphoric acid-based material at a temperature of about 100° C. to about 160° C. to obtain a blend, and mixing the blend with the benzoxazine-based monomer to obtain the mixture. 
     
     
       20. The method of  claim 17 , wherein the phosphoric acid-based material comprises at least one material selected from the group consisting of polyphosphoric acid, phosphonic acid (H 3 PO 3 ), ortho-phosphoric acid (H 3 PO 4 ), pyro-phosphoric acid (H 4 P 2 O 7 ), triphosphoric acid (H 5 P 3 O 10 ), meta-phosphoric acid, and a derivative thereof. 
     
     
       21. The method of  claim 17 , wherein the polyazole including the first repeating unit and the azole second repeating unit having at least one amino group is prepared through polymerization using a material that generates phosphoric acid when hydrolyzed. 
     
     
       22. The method of  claim 21 , wherein the material that generates phosphoric acid when hydrolyzed comprises polyphosphoric acid. 
     
     
       23. The method of  claim 17 , wherein the polyazole including the first repeating unit and the azole second repeating unit having at least one amino group is prepared by a method comprising:
 mixing biphenyl-3,3′,4,4′-tetraaminetetrahydrochloride and polyphosphoric acid, and thermally treating the mixture at a temperature of about 60 to about 250° C. to obtain a (2,2-(m-phenylene)-5,5-bibenzimidazole) oligomer; and 
 mixing the (2,2-(m-phenylene)-5,5-bibenzimidazole) oligomer with 3,4-diaminobenzoic acid and thermally treating the mixture at a temperature of about 60 to about 250° C. 
 
     
     
       24. An electrode for a fuel cell, the electrode comprising the composition of  claim 1 . 
     
     
       25. An electrolyte for a fuel cell, the electrolyte comprising the cross-linked polyazole of  claim 8 . 
     
     
       26. A fuel cell comprising:
 a cathode; 
 an anode; and 
 an electrolyte membrane according to  claim 15  disposed between the cathode and the anode. 
 
     
     
       27. A fuel cell comprising:
 a cathode; 
 an anode; and 
 an electrolyte membrane according to  claim 16  disposed between the cathode and the anode. 
 
     
     
       28. The electrolyte membrane of  claim 15 , wherein the amount of the polyazole is in the range of about 40 parts to about 210 parts by weight based on 100 parts by weight of the benzoxazine-based monomer. 
     
     
       29. The electrolyte membrane of  claim 15 , wherein L in Formula 2a is —CH 2 —, —C(CH 3 ) 2 —, or —C(CF 3 ) 2 —. 
     
     
       30. The electrolyte membrane of  claim 15 , wherein the polyazole is a block copolymer including the first repeating unit and the second repeating unit of Formula 2a. 
     
     
       31. The electrolyte membrane of  claim 15 , wherein the polyazole has a degree of polymerization of about 1 to about 900. 
     
     
       32. The electrolyte membrane of  claim 15 , wherein the polyazole comprises a block copolymer represented by Formula 3 below: 
       
         
           
           
               
               
           
         
         wherein, in Formula 3, R 1 , R 1 ′ and R 2  are hydrogen; 
         Ar is selected from among the following groups: 
       
       
         
           
           
               
               
           
         
         m is a number from 0.1 to 0.9; 
         a is 1; 
         R 3 , R 3 ′, R 3 ″, R 3 ′″, R 4 , R 4 ′, R 4 ″, R 5 , R 5 ′, and R 5 ″ are each independently a hydrogen atom, an unsubstituted or substituted C1-C20 alkyl group, an unsubstituted or substituted C1-C20 alkoxy group, an unsubstituted or substituted C6-C20 aryl group, an unsubstituted or substituted C6-C20 aryloxy group, an unsubstituted or substituted C3-C20 heteroaryl group, or an unsubstituted or substituted C3-C20 heteroaryloxy group, wherein R 1  and R 2  may be linked to form a C4-C20 carbon ring or a C3-C20 hetero ring; 
         L represents a linker; 
         n is a number from 0.1 to 0.9; and 
         k represents a degree of polymerization of the polyazole and is a number from 10 to 300. 
       
     
     
       33. The electrolyte membrane of  claim 15 , wherein the benzoxazine-based monomer comprises at least one compound selected from among the compounds represented by Formulae 6 through 11 below: 
       
         
           
           
               
               
           
         
         in Formula 6, R 1  through R 4  are each independently a hydrogen atom, a substituted or unsubstituted C 1 -C 20  alkyl group, a substituted or unsubstituted C 1 -C 20  alkoxy group, a substituted or unsubstituted C 2 -C 20  alkenyl group, a substituted or unsubstituted C 2 -C 20  alkynyl group, a substituted or unsubstituted C 6 -C 20  aryl group, a substituted or unsubstituted C 6 -C 20  aryloxy group, a substituted or unsubstituted C 2 -C 20  heteroaryl group, a substituted or unsubstituted C 2 -C 20  heteroaryloxy group, a substituted or unsubstituted C 4 -C 20  carbon ring group, a substituted or unsubstituted C 4 -C 20  carbocyclic alkyl group, a substituted or unsubstituted C 2 -C 20  heterocyclic group, a halogen atom, a hydroxyl group, or a cyano group; and 
         R 5  is a substituted or unsubstituted C 1 -C 20  alkyl group, a substituted or unsubstituted C 1 -C 20  alkoxy group, a substituted or unsubstituted C 2 -C 20  alkenyl group, a substituted or unsubstituted C 2 -C 20  alkynyl group, a substituted or unsubstituted C 6 -C 20  aryl group, a substituted or unsubstituted C 6 -C 20  aryloxy group, a substituted or unsubstituted C 7 -C 20  arylalkyl group, a substituted or unsubstituted C 2 -C 20  heteroaryl group, a substituted or unsubstituted C 2 -C 20  heteroaryloxy group, a substituted or unsubstituted C 2 -C 20  heteroarylalkyl group, a substituted or unsubstituted C 4 -C 20  carbocyclic group, a substituted or unsubstituted C 4 -C 20  carbocyclic alkyl group, a substituted or unsubstituted C 2 -C 20  heterocyclic group, or a substituted or unsubstituted C 2 -C 20  heterocyclic alkyl group, 
       
       
         
           
           
               
               
           
         
         in Formula 7, R 5 ′ is a substituted or unsubstituted C 1 -C 20  alkyl group, a substituted or unsubstituted C 1 -C 20  alkoxy group, a substituted or unsubstituted C 2 -C 20  alkenyl group, a substituted or unsubstituted C 2 -C 20  alkynyl group, a substituted or unsubstituted C 6 -C 20  aryl group, a substituted or unsubstituted C 6 -C 20  aryloxy group, a substituted or unsubstituted C 7 -C 20  arylalkyl group, a substituted or unsubstituted C 2 -C 20  heteroaryl group, a substituted or unsubstituted C 2 -C 20  heteroaryloxy group, a substituted or unsubstituted C 2 -C 20  heteroarylalkyl group, a substituted or unsubstituted C 4 -C 20  carbocyclic group, a substituted or unsubstituted C 4 -C 20  carbocyclic alkyl group, a substituted or unsubstituted C 2 -C 20  heterocyclic group, or a substituted or unsubstituted C 2 -C 20  heterocyclic alkyl group; and 
         R 6  is selected from the group consisting of a substituted or unsubstituted C 1 -C 20  alkylene group, a substituted or unsubstituted C 2 -C 20  alkenylene group, a substituted or unsubstituted C 2 -C 20  alkynylene group, a substituted or unsubstituted C 6 -C 20  arylene group, a substituted or unsubstituted C 2 -C 20  heteroarylene group, —C(═O)—, and —SO 2 —, 
       
       
         
           
           
               
               
           
         
         in Formula 8, A, B, C, D and E are all carbon; or one or two of A, B, C, D and E is nitrogen and the others are carbon; and 
         R 1  and R 2  are linked to form a ring, wherein the ring is a C 6 -C 10  carbon ring group, a C 3 -C 10  heteroaryl group, a fused C 3 -C 10  heteroaryl group, a C 3 -C 10  heterocyclic group or a fused C 3 -C 10  heterocyclic group; 
       
       
         
           
           
               
               
           
         
         in Formula 9, A is a substituted or unsubstituted C 1 -C 20  heterocyclic group, a substituted or unsubstituted C 4 -C 20  cycloalkyl group, or a substituted C 1 -C 20  alkyl group, and wherein A includes at least one oxazine moiety; and 
         R 1  through R 8  are each independently a hydrogen atom, a C 1 -C 20  alkyl group, a C 1 -C 20  alkoxy group, a C 6 -C 20  aryl group, a C 6 -C 20  aryloxy group, a C 1 -C 20  heteroaryl group, a C 1 -C 20  heteroaryloxy group, a C 4 -C 20  cycloalkyl group, a C 1 -C 20  heterocyclic group, a halogen atom, a cyano group, or a hydroxy group, 
       
       
         
           
           
               
               
           
         
         in Formula 10, R 1  and R 2  are each independently a C 1 -C 20  alkyl group, a C 1 -C 20  alkoxy group, a C 6 -C 20  aryl group, a C 6 -C 20  aryloxy group or a group represented by Formula 10A below, 
       
       
         
           
           
               
               
           
         
         in Formulae 10 and 10A, R 3  is a hydrogen atom, a C 1 -C 20  alkyl group, a C 1 -C 20  alkoxy group, a C 6 -C 20  aryl group, a C 6 -C 20  aryloxy group, a halogenated C 6 -C 20  aryl group, a halogenated C 6 -C 20  aryloxy group, a C 1 -C 20  heteroaryl group, a C 1 -C 20  heteroaryloxy group, a halogenated C 1 -C 20  heteroaryl group, a halogenated C 1 -C 20  heteroaryloxy group, a C 4 -C 20  carbon ring group, a halogenated C 4 -C 20  carbon ring group, a C 1 -C 20  heterocyclic group or a halogenated C 1 -C 20  heterocyclic group, 
       
       
         
           
           
               
               
           
         
         in Formula 11, at least two adjacent groups selected from among R 2 , R 3  and R 4  are linked to form a group represented by Formula 12A below, and the non-selected, remaining group is a hydrogen atom, a C 1 -C 20  alkyl group, a C 1 -C 20  alkoxy group, a C 6 -C 20  aryl group, a C 6 -C 20  aryloxy group, a halogenated C 6 -C 20  aryl group, a halogenated C 6 -C 20  aryloxy group, a C 1 -C 20  heteroaryl group, a C 1 -C 20  heteroaryloxy group, a halogenated C 1 -C 20  heteroaryl group, a halogenated C 1 -C 20  heteroaryloxy group, a C 4 -C 20  carbon ring group, a halogenated C 4 -C 20  carbon ring group, a C 1 -C 20  heterocyclic group or a halogenated C 1 -C 20  heterocyclic group; and 
         at least two adjacent groups selected from among R 5 , R 6  and R 7  are linked to form the group represented by Formula 12A below, and the non-selected, remaining group is a C 1 -C 20  alkyl group, a C 1 -C 20  alkoxy group, a C 6 -C 20  aryl group, a C 6 -C 20  aryloxy group, a halogenated C 6 -C 20  aryl group, a halogenated C 6 -C 20  aryloxy group, a C 1 -C 20  heteroaryl group, a C 1 -C 20  heteroaryloxy group, a halogenated C 1 -C 20  heteroaryl group, a halogenated C 1 -C 20  heteroaryloxy group, a C 4 -C 20  carbon ring group, a halogenated C 4 -C 20  carbon ring group, a C 1 -C 20  heterocyclic group or a halogenated C 1 -C 20  heterocyclic group, and 
       
       
         
           
           
               
               
           
         
         in Formula 12A, R 1  is a substituted or unsubstituted C 1 -C 20  alkyl group, a substituted or unsubstituted C 1 -C 20  alkoxy group, a substituted or unsubstituted C 2 -C 20  alkenyl group, a substituted or unsubstituted C 2 -C 20  alkynyl group, a substituted or unsubstituted C 6 -C 20  aryl group, a substituted or unsubstituted C 6 -C 20  aryloxy group, a substituted or unsubstituted C 7 -C 20  arylalkyl group, a substituted or unsubstituted C 2 -C 20  heteroaryl group, a substituted or unsubstituted C 2 -C 20  heteroaryloxy group, a substituted or unsubstituted C 2 -C 20  heteroarylalkyl group, a substituted or unsubstituted C 4 -C 20  carbon ring group, a substituted or unsubstituted C 4 -C 20  carbocyclic alkyl group, a substituted or unsubstituted C 2 -C 20  heterocyclic group, or a substituted or unsubstituted C 2 -C 20  heterocyclic alkyl group; and 
         * denotes the sites at which the at least two adjacent groups selected from among R 2 , R 3  and R 4  of Formula 11 and the at least two adjacent groups selected from among R 5 , R 6  and R 7  are linked, respectively. 
       
     
     
       34. The electrolyte membrane of  claim 16 , wherein the amount of the polyazole is in the range of about 40 parts to about 210 parts by weight based on 100 parts by weight of the benzoxazine-based monomer. 
     
     
       35. The electrolyte membrane of  claim 16 , wherein L in Formula 2a is —CH 2 —, —C(CH 3 ) 2 —, or —C(CF 3 ) 2 —. 
     
     
       36. The electrolyte membrane of  claim 16 , wherein the polyazole is a block copolymer including the first repeating unit and the second repeating unit of Formula 2a. 
     
     
       37. The electrolyte membrane of  claim 16 , wherein the polyazole has a degree of polymerization of about 1 to about 900. 
     
     
       38. The electrolyte membrane of  claim 16 , wherein the polyazole comprises a block copolymer represented by Formula 3 below: 
       
         
           
           
               
               
           
         
         wherein, in Formula 3, R 1 , R 1 ′ and R 2  are hydrogen; Ar is selected from among the following groups: 
       
       
         
           
           
               
               
           
         
         m is a number from 0.1 to 0.9; 
         a is 1; 
         R 3 , R 3 ′, R 3 ″, R 3 ′″, R 4 , R 4 ′, R 4 ″, R 5 , R 5 ′, and R 5 ″ are each independently a hydrogen atom, an unsubstituted or substituted C1-C20 alkyl group, an unsubstituted or substituted C1-C20 alkoxy group, an unsubstituted or substituted C6-C20 aryl group, an unsubstituted or substituted C6-C20 aryloxy group, an unsubstituted or substituted C3-C20 heteroaryl group, or an unsubstituted or substituted C3-C20 heteroaryloxy group, wherein R 1  and R 2  may be linked to form a C4-C20 carbon ring or a C3-C20 hetero ring; 
         L represents a linker; 
         n is a number from 0.1 to 0.9; and 
         k represents a degree of polymerization of the polyazole and is a number from 10 to 300. 
       
     
     
       39. The electrolyte membrane of  claim 16 , wherein the benzoxazine-based monomer comprises at least one compound selected from among the compounds represented by Formulae 6 through 11 below: 
       
         
           
           
               
               
           
         
         in Formula 6, R 1  through R 4  are each independently a hydrogen atom, a substituted or unsubstituted C 1 -C 20  alkyl group, a substituted or unsubstituted C 1 -C 20  alkoxy group, a substituted or unsubstituted C 2 -C 20  alkenyl group, a substituted or unsubstituted C 2 -C 20  alkynyl group, a substituted or unsubstituted C 6 -C 20  aryl group, a substituted or unsubstituted C 6 -C 20  aryloxy group, a substituted or unsubstituted C 2 -C 20  heteroaryl group, a substituted or unsubstituted C 2 -C 20  heteroaryloxy group, a substituted or unsubstituted C 4 -C 20  carbon ring group, a substituted or unsubstituted C 4 -C 20  carbocyclic alkyl group, a substituted or unsubstituted C 2 -C 20  heterocyclic group, a halogen atom, a hydroxyl group, or a cyano group; and 
         R 5  is a substituted or unsubstituted C 1 -C 20  alkyl group, a substituted or unsubstituted C 1 -C 20  alkoxy group, a substituted or unsubstituted C 2 -C 20  alkenyl group, a substituted or unsubstituted C 2 -C 20  alkynyl group, a substituted or unsubstituted C 6 -C 20  aryl group, a substituted or unsubstituted C 6 -C 20  aryloxy group, a substituted or unsubstituted C 7 -C 20  arylalkyl group, a substituted or unsubstituted C 2 -C 20  heteroaryl group, a substituted or unsubstituted C 2 -C 20  heteroaryloxy group, a substituted or unsubstituted C 2 -C 20  heteroarylalkyl group, a substituted or unsubstituted C 4 -C 20  carbocyclic group, a substituted or unsubstituted C 4 -C 20  carbocyclic alkyl group, a substituted or unsubstituted C 2 -C 20  heterocyclic group, or a substituted or unsubstituted C 2 -C 20  heterocyclic alkyl group, 
       
       
         
           
           
               
               
           
         
         in Formula 7, R 5 ′ is a substituted or unsubstituted C 1 -C 20  alkyl group, a substituted or unsubstituted C 1 -C 20  alkoxy group, a substituted or unsubstituted C 2 -C 20  alkenyl group, a substituted or unsubstituted C 2 -C 20  alkynyl group, a substituted or unsubstituted C 6 -C 20  aryl group, a substituted or unsubstituted C 6 -C 20  aryloxy group, a substituted or unsubstituted C 7 -C 20  arylalkyl group, a substituted or unsubstituted C 2 -C 20  heteroaryl group, a substituted or unsubstituted C 2 -C 20  heteroaryloxy group, a substituted or unsubstituted C 2 -C 20  heteroarylalkyl group, a substituted or unsubstituted C 4 -C 20  carbocyclic group, a substituted or unsubstituted C 4 -C 20  carbocyclic alkyl group, a substituted or unsubstituted C 2 -C 20  heterocyclic group, or a substituted or unsubstituted C 2 -C 20  heterocyclic alkyl group; and 
         R 6  is selected from the group consisting of a substituted or unsubstituted C 1 -C 20  alkylene group, a substituted or unsubstituted C 2 -C 20  alkenylene group, a substituted or unsubstituted C 2 ′ C 20  alkynylene group, a substituted or unsubstituted C 6 -C 20  arylene group, a substituted or unsubstituted C 2 -C 20  heteroarylene group, —C(═O)—, and —SO 2 —, 
       
       
         
           
           
               
               
           
         
         in Formula 8, A, B, C, D and E are all carbon; or one or two of A, B, C, D and E is nitrogen and the others are carbon; and 
         R 1  and R 2  are linked to form a ring, wherein the ring is a C 6 -C 10  carbon ring group, a C 3 -C 10  heteroaryl group, a fused C 3 -C 10  heteroaryl group, a C 3 -C 10  heterocyclic group or a fused C 3 -C 10  heterocyclic group; 
       
       
         
           
           
               
               
           
         
         in Formula 9, A is a substituted or unsubstituted C 1 -C 20  heterocyclic group, a substituted or unsubstituted C 4 -C 20  cycloalkyl group, or a substituted C 1 -C 20  alkyl group, and wherein A includes at least one oxazine moiety; and 
         R 1  through R 8  are each independently a hydrogen atom, a C 1 -C 20  alkyl group, a C 1 -C 20  alkoxy group, a C 6 -C 20  aryl group, a C 6 -C 20  aryloxy group, a C 1 -C 20  heteroaryl group, a C 1 -C 20  heteroaryloxy group, a C 4 -C 20  cycloalkyl group, a C 1 -C 20  heterocyclic group, a halogen atom, a cyano group, or a hydroxy group, 
       
       
         
           
           
               
               
           
         
         in Formula 10, R 1  and R 2  are each independently a C 1 -C 20  alkyl group, a C 1 -C 20  alkoxy group, a C 6 -C 20  aryl group, a C 6 -C 20  aryloxy group or a group represented by Formula 10A below, 
       
       
         
           
           
               
               
           
         
         in Formulae 10 and 10A, R 3  is a hydrogen atom, a C 1 -C 20  alkyl group, a C 1 -C 20  alkoxy group, a C 6 -C 20  aryl group, a C 6 -C 20  aryloxy group, a halogenated C 6 -C 20  aryl group, a halogenated C 6 -C 20  aryloxy group, a C 1 -C 20  heteroaryl group, a C 1 -C 20  heteroaryloxy group, a halogenated C 1 -C 20  heteroaryl group, a halogenated C 1 -C 20  heteroaryloxy group, a C 4 -C 20  carbon ring group, a halogenated C 4 -C 20  carbon ring group, a C 1 -C 20  heterocyclic group or a halogenated C 1 -C 20  heterocyclic group, 
       
       
         
           
           
               
               
           
         
         in Formula 11, at least two adjacent groups selected from among R 2 , R 3  and R 4  are linked to form a group represented by Formula 12A below, and the non-selected, remaining group is a hydrogen atom, a C 1 -C 20  alkyl group, a C 1 -C 20  alkoxy group, a C 6 -C 20  aryl group, a C 6 -C 20  aryloxy group, a halogenated C 6 -C 20  aryl group, a halogenated C 6 -C 20  aryloxy group, a C 1 -C 20  heteroaryl group, a C 1 -C 20  heteroaryloxy group, a halogenated C 1 -C 20  heteroaryl group, a halogenated C 1 -C 20  heteroaryloxy group, a C 4 -C 20  carbon ring group, a halogenated C 4 -C 20  carbon ring group, a C 1 -C 20  heterocyclic group or a halogenated C 1 -C 20  heterocyclic group; and 
         at least two adjacent groups selected from among R 5 , R 6  and R 7  are linked to form the group represented by Formula 12A below, and the non-selected, remaining group is a C 1 -C 20  alkyl group, a C 1 -C 20  alkoxy group, a C 6 -C 20  aryl group, a C 6 -C 20  aryloxy group, a halogenated C 6 -C 20  aryl group, a halogenated C 6 -C 20  aryloxy group, a C 1 -C 20  heteroaryl group, a C 1 -C 20  heteroaryloxy group, a halogenated C 1 -C 20  heteroaryl group, a halogenated C 1 -C 20  heteroaryloxy group, a C 4 -C 20  carbon ring group, a halogenated C 4 -C 20  carbon ring group, a C 1 -C 20  heterocyclic group or a halogenated C 1 -C 20  heterocyclic group, and 
       
       
         
           
           
               
               
           
         
         in Formula 12A, R 1  is a substituted or unsubstituted C 1 -C 20  alkyl group, a substituted or unsubstituted C 1 -C 20  alkoxy group, a substituted or unsubstituted C 2 -C 20  alkenyl group, a substituted or unsubstituted C 2 -C 20  alkynyl group, a substituted or unsubstituted C 6 -C 20  aryl group, a substituted or unsubstituted C 6 -C 20  aryloxy group, a substituted or unsubstituted C 7 -C 20  arylalkyl group, a substituted or unsubstituted C 2 -C 20  heteroaryl group, a substituted or unsubstituted C 2 -C 20  heteroaryloxy group, a substituted or unsubstituted C 2 -C 20  heteroarylalkyl group, a substituted or unsubstituted C 4 -C 20  carbon ring group, a substituted or unsubstituted C 4 -C 20  carbocyclic alkyl group, a substituted or unsubstituted C 2 -C 20  heterocyclic group, or a substituted or unsubstituted C 2 -C 20  heterocyclic alkyl group; and 
         * denotes the sites at which the at least two adjacent groups selected from among R 2 , R 3  and R 4  of Formula 11 and the at least two adjacent groups selected from among R 5 , R 6  and R 7  are linked, respectively. 
       
     
     
       40. The membrane of  claim 15 , wherein the molar ratio of the first repeating unit to the second repeating unit is about 8:2, about 5:5, or about 2:8. 
     
     
       41. The membrane of  claim 16 , wherein the molar ratio of the first repeating unit to the second repeating unit is about 8:2, about 5:5, or about 2:8. 
     
     
       42. The membrane of  claim 16 , wherein the benzoxazine-based monomer comprises at least one compound selected from among the compounds represented by Formulae 6 through 11: 
       
         
           
           
               
               
           
         
         in Formula 6, R 1 , R 2  and R 4  are each independently a hydrogen atom, a substituted or unsubstituted C 1 -C 20  alkyl group, a substituted or unsubstituted C 1 -C 20  alkoxy group, a substituted or unsubstituted C 2 -C 20  alkenyl group, a substituted or unsubstituted C 2 -C 20  alkynyl group, a substituted or unsubstituted C 6 -C 20  aryl group, a substituted or unsubstituted C 6 -C 20  aryloxy group, a substituted or unsubstituted C 2 -C 20  heteroaryl group, a substituted or unsubstituted C 2 -C 20  heteroaryloxy group, a substituted or unsubstituted C 4 -C 20  carbon ring group, a substituted or unsubstituted C 4 -C 20  carbocyclic alkyl group, a substituted or unsubstituted C 2 -C 20  heterocyclic group, a halogen atom, a hydroxyl group, or a cyano group; 
         R 3  is independently a substituted or unsubstituted C 1 -C 20  alkoxy group, a substituted or unsubstituted C 2 -C 20  alkenyl group, a substituted or unsubstituted C 2 -C 20  alkynyl group, a substituted or unsubstituted C 6 -C 20  aryloxy group, a substituted or unsubstituted C 2 -C 20  heteroaryloxy group, a substituted or unsubstituted C 4 -C 20  carbocyclic alkyl group, a halogen atom, a hydroxyl group, or a cyano group; and 
         R 5  is a substituted or unsubstituted C 1 -C 20  alkyl group, a substituted or unsubstituted C 1 -C 20  alkoxy group, a substituted or unsubstituted C 2 -C 20  alkenyl group, a substituted or unsubstituted C 2 -C 20  alkynyl group, a substituted or unsubstituted C 6 -C 20  aryl group, a substituted or unsubstituted C 6 -C 20  aryloxy group, a substituted or unsubstituted C 7 -C 20  arylalkyl group, a substituted or unsubstituted C 2 -C 20  heteroaryl group, a substituted or unsubstituted C 2 -C 20  heteroaryloxy group, a substituted or unsubstituted C 2 -C 20  heteroarylalkyl group, a substituted or unsubstituted C 4 -C 20  carbocyclic group, a substituted or unsubstituted C 4 -C 20  carbocyclic alkyl group, a substituted or unsubstituted C 2 -C 20  heterocyclic group, or a substituted or unsubstituted C 2 -C 20  heterocyclic alkyl group, 
       
       
         
           
           
               
               
           
         
         in Formula 7, R 5 ′ is a substituted or unsubstituted C 1 -C 20  alkoxy group, a substituted or unsubstituted C 6 -C 20  aryloxy group, or a substituted or unsubstituted C 2 -C 20  heteroaryloxy group; and 
         R 6  is selected from the group consisting of a substituted or unsubstituted C 1 -C 20  alkylene group, a substituted or unsubstituted C 2 -C 20  alkenylene group, a substituted or unsubstituted C 2 -C 20  alkynylene group, a substituted or unsubstituted C 6 -C 20  arylene group, a substituted or unsubstituted C 2 -C 20  heteroarylene group, —C(═O)—, and —SO 2 —, 
       
       
         
           
           
               
               
           
         
         in Formula 8, A, B, C, D and E are all carbon; or one or two of A, B, C, D and E is nitrogen and the others are carbon; and 
         R 1  and R 2  are linked to form a ring, wherein the ring is a C 6 -C 10  carbon ring group, a C 3 -C 10  heteroaryl group, a fused C 3 -C 10  heteroaryl group, a C 3 -C 10  heterocyclic group or a fused C 3 -C 10  heterocyclic group; 
       
       
         
           
           
               
               
           
         
         in Formula 9, A is a substituted or unsubstituted C 1 -C 20  heterocyclic group, a substituted or unsubstituted C 4 -C 20  cycloalkyl group, or a substituted C 1 -C 20  alkyl group, and wherein A includes at least one oxazine moiety; and 
         R 1  through R 8  are each independently a hydrogen atom, a C 1 -C 20  alkyl group, a C 1 -C 20  alkoxy group, a C 6 -C 20  aryl group, a C 6 -C 20  aryloxy group, a C 1 -C 20  heteroaryl group, a C 1 -C 20  heteroaryloxy group, a C 4 -C 20  cycloalkyl group, a C 1 -C 20  heterocyclic group, a halogen atom, a cyano group, or a hydroxy group, 
       
       
         
           
           
               
               
           
         
         in Formula 10, R 1  and R 2  are each independently a C 1 -C 20  alkyl group, a C 1 -C 20  alkoxy group, a C 6 -C 20  aryl group, a C 6 -C 20  aryloxy group or a group represented by Formula 10A below, 
       
       
         
           
           
               
               
           
         
         in Formulae 10 and 10A, R 3  is a hydrogen atom, a C 1 -C 20  alkyl group, a C 1 -C 20  alkoxy group, a C 6 -C 20  aryl group, a C 6 -C 20  aryloxy group, a halogenated C 6 -C 20  aryl group, a halogenated C 6 -C 20  aryloxy group, a C 1 -C 20  heteroaryl group, a C 1 -C 20  heteroaryloxy group, a halogenated C 1 -C 20  heteroaryl group, a halogenated C 1 -C 20  heteroaryloxy group, a C 4 -C 20  carbon ring group, a halogenated C 4 -C 20  carbon ring group, a C 1 -C 20  heterocyclic group or a halogenated C 1 -C 20  heterocyclic group, 
       
       
         
           
           
               
               
           
         
         in Formula 11, at least two adjacent groups selected from among R 2 , R 3  and R 4  are linked to form a group represented by Formula 12A below, and the non-selected, remaining group is a hydrogen atom, a C 1 -C 20  alkyl group, a C 1 -C 20  alkoxy group, a C 6 -C 20  aryl group, a C 6 -C 20  aryloxy group, a halogenated C 6 -C 20  aryl group, a halogenated C 6 -C 20  aryloxy group, a C 1 -C 20  heteroaryl group, a C 1 -C 20  heteroaryloxy group, a halogenated C 1 -C 20  heteroaryl group, a halogenated C 1 -C 20  heteroaryloxy group, a C 4 -C 20  carbon ring group, a halogenated C 4 -C 20  carbon ring group, a C 1 -C 20  heterocyclic group or a halogenated C 1 -C 20  heterocyclic group; and 
         at least two adjacent groups selected from among R 5 , R 6  and R 7  are linked to form the group represented by Formula 12A below, and the non-selected, remaining group is a C 1 -C 20  alkyl group, a C 1 -C 20  alkoxy group, a C 6 -C 20  aryl group, a C 6 -C 20  aryloxy group, a halogenated C 6 -C 20  aryl group, a halogenated C 6 -C 20  aryloxy group, a C 1 -C 20  heteroaryl group, a C 1 -C 20  heteroaryloxy group, a halogenated C 1 -C 20  heteroaryl group, a halogenated C 1 -C 20  heteroaryloxy group, a C 4 -C 20  carbon ring group, a halogenated C 4 -C 20  carbon ring group, a C 1 -C 20  heterocyclic group or a halogenated C 1 -C 20  heterocyclic group, and 
       
       
         
           
           
               
               
           
         
         in Formula 12A, R 1  is a substituted or unsubstituted C 1 -C 20  alkyl group, a substituted or unsubstituted C 1 -C 20  alkoxy group, a substituted or unsubstituted C 2 -C 20  alkenyl group, a substituted or unsubstituted C 2 -C 20  alkynyl group, a substituted or unsubstituted C 6 -C 20  aryl group, a substituted or unsubstituted C 6 -C 20  aryloxy group, a substituted or unsubstituted C 7 -C 20  arylalkyl group, a substituted or unsubstituted C 2 -C 20  heteroaryl group, a substituted or unsubstituted C 2 -C 20  heteroaryloxy group, a substituted or unsubstituted C 2 -C 20  heteroarylalkyl group, a substituted or unsubstituted C 4 -C 20  carbon ring group, a substituted or unsubstituted C 4 -C 20  carbocyclic alkyl group, a substituted or unsubstituted C 2 -C 20  heterocyclic group, or a substituted or unsubstituted C 2 -C 20  heterocyclic alkyl group; and 
         * denotes the sites at which the at least two adjacent groups selected from among R 2 , R 3  and R 4  of Formula 11 and the at least two adjacent groups selected from among R 5 , R 6  and R 7  are linked, respectively. 
       
     
     
       43. An electrolyte membrane for a fuel cell, the electrolyte membrane comprising a cross-linked polyazole obtained through a cross-linking reaction of a composition comprising: a polyazole including a first repeating unit comprising a repeating unit represented by one of the following formulae: 
       
         
           
           
               
               
           
         
         wherein Ar is selected from among the following groups: 
       
       
         
           
           
               
               
           
         
       
       an azole second repeating unit; and a benzoxazine-based monomer, wherein, assuming that m and n represent the relative molar amount of the first repeating unit and the azole second repeating unit, respectively, in the polyazole such that m+n=1, m is a number from 0.1 to 0.9 and n is a number from 0.1 to 0.9:
 wherein the azole second repeating unit comprises a repeating unit represented by Formula 2a: 
 
       
         
           
           
               
               
           
         
         wherein, in Formula 2a, R 3 , R 3 ′, R 3 ″, R 3 ′″, R 4 , R 4 ′, R 4 ″, R 5 , R 5 ′, and R 5 ″ are each independently a hydrogen atom, an unsubstituted or substituted C1-C20 alkyl group, an unsubstituted or substituted C1-C20 alkoxy group, an unsubstituted or substituted C6-C20 aryl group, an unsubstituted or substituted C6-C20 aryloxy group, an unsubstituted or substituted C3-C20 heteroaryl group, or an unsubstituted or substituted C3-C20 heteroaryloxy group, wherein R 1  and R 2  may be linked to form a C4-C20 carbon ring or a C3-C20 hetero ring; and 
         L represents a linker, and 
       
       wherein the benzoxazine-based monomer comprises at least one compound selected from:

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